Marcelino has “ceased to be the coach of Villarreal”, according to a statement on the club’s official website.
The news comes after Marcelino led Villarreal to a fourth-place finish in La Liga last season to clinch the club’s return to the Champions League after an eight-year exile, and also reached the semi-finals of the Europa League.
Marcelino joined the club in January 2013, securing promotion to La Liga later that season with a second-place finish in Segunda Division, helping him to earn a two-year contract later that year.
Villarreal finished sixth in 2013-14 and qualified for the Europa League, and Marcelino repeated that feat the following season.
A statement on the club’s official website said: “Marcelino Garcia Toral has ceased to be the coach of Villarreal CF. The club wishes to thank the coach, the coach, Ruben Uria, and trainer Ismael Fernandez.
“His work in these three-and-a-half seasons in front of the yellow bench, where they have achieved great success with a return to the first division rankings, Europa League semi-finals, and the Europa League and fourth place last season to qualify for the Champions League.
“Villarreal CF wants to wish the best to Marcelino in his career. In the coming hours the replacement will be announced on an interim or final basis.”